Catalytic applications of MCM-41 with different pore sizes in selected liquid phase reactions

被引:73
作者
Choi, JS [1 ]
Kim, DJ [1 ]
Chang, SH [1 ]
Ahn, WS [1 ]
机构
[1] Inha Univ, Sch Chem Sci & Engn, Inchon 402751, South Korea
关键词
MCM-41; pore-size effect; Ti-grafting; Mn-salen complex; sulfonic acid immobilization;
D O I
10.1016/S0926-860X(03)00485-X
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 [物理化学]; 081704 [应用化学];
摘要
A series of MCM-41 with pore diameters in 20-90 Angstrom range was prepared and the effects of pore size on liquid phase reactions of epoxidation, etherification, and esterification were investigated after Ti-grafting, immobilization of Mn-salen complex, and monolayer adsorption Of SO3H were performed on the host materials, respectively. Amount of functionalized species increased with the pore diameters of MCM-41, but it leveled off after a thresh hold pore size is attained. MCM-41 with pore diameter of ca. 56 Angstrom was recommended to obtain high concentration of grafted species with good catalytic performances. In cyclohexene epoxidation, conversion showed linear relationship with Ti-contents of the catalyst, which proved to be a primary factor governing the reaction rather than diffusion effect. For MCM-41 immobilized with Mn-salen complexes, active site isolation in high surface coverage was required for good catalytic performances. MCM-41 with enlarged pores was again better for larger amount of thiol group to be attached to the mesopore surfaces, but uniform surface property/shape seems also required to promote the formation of a monolayer-type coated material. Esteritication of 1-propanol with hexanoic acid was best catalyzed by the acidity of the sulfone-functionalized MCM-41 materials synthesized after 12 h oxidation treatment of the thiol-grafted MCM-41. (C) 2003 Elsevier B.V. All rights reserved.
引用
收藏
页码:225 / 237
页数:13
相关论文
共 31 条
[1]
Synthesis, characterization, and catalytic properties of Ti-containing mesoporous molecular sieves prepared using a fluorosilicon compound [J].
Ahn, WS ;
Kim, NK ;
Jeong, SY .
CATALYSIS TODAY, 2001, 68 (1-3) :83-88
[2]
Transition-metal ligands bound onto the micelle-templated silica surface [J].
Brunel, D ;
Bellocq, N ;
Sutra, P ;
Cauvel, A ;
Laspéras, M ;
Moreau, P ;
Di Renzo, F ;
Galarneau, A ;
Fajula, F .
COORDINATION CHEMISTRY REVIEWS, 1998, 178 :1085-1108
[3]
Iron and copper immobilised on mesoporous MCM-41 molecular sieves as catalysts for the oxidation of cyclohexane [J].
Carvalho, WA ;
Wallau, M ;
Schuchardt, U .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 1999, 144 (01) :91-99
[4]
Epoxidations of olefins catalysed by new Mn(II) salen immobilized mesoporous materials [J].
Choudary, BM ;
Kantam, ML ;
Bharathi, B ;
Sreekanth, P ;
Figueras, F .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2000, 159 (02) :417-421
[5]
DESPLANTIERGISC.D, 2001, STUD SURF SCI CATAL, V135, P205
[6]
The oxidation of alkenes in the presence of some transition metal elements exchanged with zeolites [J].
Farzaneh, F ;
Sadeghi, S ;
Turkian, L ;
Ghandi, M .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 1998, 132 (2-3) :255-261
[7]
Functionalized monolayers on ordered mesoporous supports [J].
Feng, X ;
Fryxell, GE ;
Wang, LQ ;
Kim, AY ;
Liu, J ;
Kemner, KM .
SCIENCE, 1997, 276 (5314) :923-926
[8]
DRS UV-VIS AND EPR SPECTROSCOPY OF HYDROPEROXO AND SUPEROXO COMPLEXES IN TITANIUM SILICALITE [J].
GEOBALDO, F ;
BORDIGA, S ;
ZECCHINA, A ;
GIAMELLO, E ;
LEOFANTI, G ;
PETRINI, G .
CATALYSIS LETTERS, 1992, 16 (1-2) :109-115
[9]
HUO Q, 1996, CHEM MATER, V8, P1447
[10]
Comprehensive characterization of highly ordered MCM-41 silicas using nitrogen adsorption, thermogravimetry, X-ray diffraction and transmission electron microscopy [J].
Jaroniec, M ;
Kruk, M ;
Shin, HJ ;
Ryoo, R ;
Sakamoto, Y ;
Terasaki, O .
MICROPOROUS AND MESOPOROUS MATERIALS, 2001, 48 (1-3) :127-134